EP1421630B1 - Abscheidungsverfahren von einer oxydschicht auf einem substrat und dieses verwendende photovoltaische zelle - Google Patents

Abscheidungsverfahren von einer oxydschicht auf einem substrat und dieses verwendende photovoltaische zelle Download PDF

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Publication number
EP1421630B1
EP1421630B1 EP02754092A EP02754092A EP1421630B1 EP 1421630 B1 EP1421630 B1 EP 1421630B1 EP 02754092 A EP02754092 A EP 02754092A EP 02754092 A EP02754092 A EP 02754092A EP 1421630 B1 EP1421630 B1 EP 1421630B1
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EP
European Patent Office
Prior art keywords
substrate
chamber
depositing
oxide layer
sources
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Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
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EP02754092A
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English (en)
French (fr)
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EP1421630A2 (de
Inventor
Ulrich Kroll
Johannes Meier
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Universite de Neuchatel
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Universite de Neuchatel
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/18—Processes or apparatus specially adapted for the manufacture or treatment of these devices or of parts thereof
    • H01L31/1884—Manufacture of transparent electrodes, e.g. TCO, ITO
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/04—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices
    • H01L31/06—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices characterised by potential barriers
    • H01L31/075—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices characterised by potential barriers the potential barriers being only of the PIN type, e.g. amorphous silicon PIN solar cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/50—Photovoltaic [PV] energy
    • Y02E10/548—Amorphous silicon PV cells

Definitions

  • the present invention relates to a method of depositing a transparent oxide layer on a substrate, which is particularly applicable to the manufacture of a photovoltaic cell, also called solar cell.
  • the invention also relates to such a cell whose transparent oxide layer is deposited according to this method.
  • the most technologically advanced solar cells comprise a substrate, a transparent conductive oxide (TCO) conductive oxide layer deposited on the substrate and a photovoltaically active layer deposited on the oxide layer.
  • This photosensitive layer is advantageously composed of three sub-layers of amorphous hydrogenated silicon, microcrystalline or nanocrystalline forming a p-i-n junction. More precisely, the two external sublayers are respectively positively and negatively doped, while the intermediate sublayer is intrinsic.
  • a cell of this type is described in detail, for example, according to several embodiments, in WO 97/24769.
  • US-A-5,002,796 discloses a method for depositing a transparent conductive oxide layer which consists in providing sources containing an oxygen-based liquid compound.
  • photovoltaic cells generally use a transparent conductive oxide layer made of tin dioxide (SnO 2 ) or zinc oxide (ZnO) deposited on a glass substrate by the chemical vaporization process. known under the abbreviation CVD (Chemical Vapor Deposition), which is carried out at a temperature generally between 400 and 550 ° C.
  • CVD Chemical Vapor Deposition
  • U.S. Patent No. 5,252,140 discloses a solar cell on tempered glass in which the soaking is performed after formation of the oxide layer. To avoid degradation thereof, heating is carried out at 650 ° C maximum for less than 2 minutes, before being rapidly cooled by air. These precautions, however, increase the process and do not guarantee the quality of the soaking.
  • US Pat. Nos. 4,751,149 and 5,002,796 disclose methods of depositing the vapor phase oxide layer in which the chemical compounds participating in the reaction are brought to the chamber by a carrier gas saturated with these compounds by bubbling.
  • Such a method makes it possible, of course, to have softer reaction conditions, which do not alter the properties of the substrate, and therefore to be used, in particular, for the production of solar cells on tempered glass.
  • the method does not allow good control of the amount of reagents involved, because the thermodynamic equilibrium that governs the saturation threshold of the carrier gas strongly depends on the temperature and the flow of this gas. Since it is problematic to precisely set the temperature in the entire circuit, there is a risk of uncontrolled recondensation of reagents in a colder place of the installation. The regularity and reproducibility of the layer are, therefore, quite difficult to ensure.
  • the chemical vaporization is carried out in a plasma of the deposition gases, formed inside the pregnant, preferably using the technique of PECVD (Plasma Enhanced Chemical Vapor Deposition), well known to those skilled in the art.
  • PECVD Pulsma Enhanced Chemical Vapor Deposition
  • the active layer of the cell comprises three sub-layers of amorphous, microcrystalline or nanocrystalline hydrogenated silicon forming a p-i-n junction, the two external sublayers being respectively positively and negatively doped.
  • the substrate is made of glass, preferably tempered glass, but it can also be made of stainless steel, aluminum or a polymer.
  • the cell shown in FIG. 1 uses as substrate a thin tempered glass plate, having a thickness of the order of 1 to 8 mm, on which is deposited a transparent conductive oxide (TCO) layer 12 having, typically, a thickness of 0.2 to 4 ⁇ m.
  • TCO transparent conductive oxide
  • the layer 12 advantageously consisting of tin dioxide (SnO 2 ), zinc oxide (ZnO) or an oxide of tin and zinc, is deposited by chemical vaporization (CVD) according to a process which will be described further.
  • a photovoltaic active layer 14 having a thickness of about 0.2 to 10 ⁇ m, is deposited on the oxide layer 12. It is composed of three sublayers of amorphous hydrogenated silicon, microcrystalline or nanocrystalline 16, 18 and 20, forming a pine junction. The two outer sublayers 16 and 20 are respectively positively and negatively doped.
  • the cell further comprises a rear contact layer 22, for example zinc oxide, deposited on the active layer 14 and a reflective layer 24, for example silver or aluminum, deposited on the layer 22.
  • a rear contact layer 22 for example zinc oxide
  • a reflective layer 24 for example silver or aluminum
  • FIG. 2 shows the equipment for the CVD deposition of a layer of zinc oxide 12 on the tempered glass plate 10.
  • a sealed chamber with a heating support 28 on which is deposited the tempered glass plate.
  • the chamber 26 is connected to a vacuum pump 30 and three reservoirs 32, 34 and 36 containing, first, water, the second, diethyl (C 2 H 5 ) 2 Zn and the third, a dopant, advantageously in the form of diborane (B 2 H 6 ).
  • B 2 H 6 diborane
  • the contents of the two tanks 32 and 34 are liquid, while that of the tank 36 is a gaseous mixture of 0.5 to 2% of diborane diluted in a gas such as nitrogen, argon or hydrogen. It will be noted that the tanks 32 and 34 are connected directly to the enclosure.
  • the reservoir 36 is pre-connected to the supply conduit of the reservoir 34, but it can also be connected directly to the enclosure.
  • the enclosure 26 is carried, using the heating support 28, at a temperature of about 180 ° C, but may be between 130 and 300 ° C, while the pump 30 lowers the pressure at a value of 0.3 to 0.5 mbar, but which can be between 0.01 and 20 mbar.
  • the adjustable valves (not shown) connecting the reservoirs 32, 34 and 36 to the enclosure 26 are then open.
  • the diethylzinc and the water contained therein in the liquid state evaporate on their surface and the resulting gases sucked into the chamber, react with each other and with the doping gas (B 2 H 6 ) to cause, at the temperature of the substrate, according to a known reaction, the deposition of the desired zinc oxide layer 12 on the tempered glass plate 10.
  • the tempered glass Since the operation takes place at a relatively low temperature, the tempered glass undergoes no deterioration of its properties. Moreover, given the homogeneous and low pressure prevailing in the installation, the gases sprays are not likely to recondense before admission to the enclosure.
  • the above method is ideal for depositing zinc oxide doped with diborane because the chemical reactions involved are without problems at the temperatures mentioned.
  • a CVD deposition of tin dioxide or a deposit of zinc oxide with a more stable dopant such as methyl tetrafluoride (CF 4 ) these temperatures are too low for that the reactions take place normally.
  • the deposition of the oxide layer is then carried out by the PECVD plasma chemical vaporization method.
  • the enclosure 26 is equipped with an electrode, for example in the form of a grid 38, disposed above the heating support 28 and an electric generator 40 is connected between this electrode and the support.
  • the gases introduced into the chamber 26 give rise to the formation of a plasma between the electrode 38 and the support 28. Active radicals are thus generated by the plasma and allow the chemical reactions giving rise to the deposition of the oxide layer to be at a temperature substantially lower than that normally required, thus preserving the properties of the substrate.
  • the tanks 34 and 36 respectively contain, for example, tetramethyltin (CH 3 ) 4 Sn and, as a dopant, methyl tetrafluoride (CF 4 ). It goes without saying that other compounds, well known in the art, can be used.
  • the water in the reservoir 32 may be replaced by any oxygen-containing compound (N 2 O, CH 3 OH, C 2 H 5 OH, ...) and that the dopant contained in the reservoir 36 may also be be in liquid form.

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  • Engineering & Computer Science (AREA)
  • Computer Hardware Design (AREA)
  • Physics & Mathematics (AREA)
  • Condensed Matter Physics & Semiconductors (AREA)
  • Electromagnetism (AREA)
  • General Physics & Mathematics (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Power Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Chemical Vapour Deposition (AREA)
  • Photovoltaic Devices (AREA)
  • Chemically Coating (AREA)
  • Manufacturing Of Electric Cables (AREA)
  • Hybrid Cells (AREA)

Claims (5)

  1. Verfahren zur Abscheidung einer Schicht (12) aus transparentem leitfähigem Oxid auf einem in einer Kammer (26) angeordneten Substrat (10), dadurch gekennzeichnet, daß:
    - Quellen (32, 34, 36), die eine flüssige Verbindung auf Basis von Sauerstoff, eine flüssige Verbindung des zur Bildung des Oxids vorgesehenen Metalls bzw. einen Dotierstoff in gasförmiger oder flüssiger Form enthalten, bereitgestellt werden,
    - in der Kammer eine Temperatur zwischen 130 und 300°C und ein Druck zwischen 0,01 und 2 mbar eingestellt wird und dann
    - die Quellen mit der Kammer in Verbindung gebracht werden, wodurch die Flüssigkeiten an ihrer Oberfläche verdampfen, in die Kammer gesaugt werden, ohne daß die Verwendung eines Trägergases notwendig ist, und dort mit dem Dotierstoff unter Ausbildung der Oxidschicht auf dem Substrat reagieren.
  2. Verfahren nach Anspruch 1 zur Abscheidung einer Zinkoxidschicht, dadurch gekennzeichnet, daß die Quellen (32, 34, 36) Wasser, Diethylzink in flüssiger Form bzw. ein Gasgemisch auf Basis von Diboran enthalten.
  3. Verfahren nach Anspruch 1, dadurch gekennzeichnet, daß dabei außerdem ein Plasma der in der Kammer verdampften Flüssigkeiten gebildet wird.
  4. Verfahren nach Anspruch 3 zur Abscheidung einer Zinnoxidschicht, dadurch gekennzeichnet, daß die Quellen (32, 34, 36) Wasser, Tetramethylzinn in flüssiger Form bzw. ein Gasgemisch auf Basis von Tetrafluormethan enthalten.
  5. Verfahren nach Anspruch 3 zur Abscheidung einer Zinkoxidschicht, dadurch gekennzeichnet, daß die Quellen (32, 34, 36) Wasser, Diethylzink in flüssiger Form bzw. ein Gasgemisch auf Basis von Tetrafluormethan enthalten.
EP02754092A 2001-08-30 2002-08-23 Abscheidungsverfahren von einer oxydschicht auf einem substrat und dieses verwendende photovoltaische zelle Expired - Lifetime EP1421630B1 (de)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP02754092A EP1421630B1 (de) 2001-08-30 2002-08-23 Abscheidungsverfahren von einer oxydschicht auf einem substrat und dieses verwendende photovoltaische zelle

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
EP01810840A EP1289025A1 (de) 2001-08-30 2001-08-30 Abscheidungsverfahren von einer Oxydschicht auf einem Substrat und dieses verwendende photovoltaische Zelle
EP01810840 2001-08-30
EP02754092A EP1421630B1 (de) 2001-08-30 2002-08-23 Abscheidungsverfahren von einer oxydschicht auf einem substrat und dieses verwendende photovoltaische zelle
PCT/CH2002/000458 WO2003021690A2 (fr) 2001-08-30 2002-08-23 Procede de depot d'une couche d'oxyde sur un substrat et cellule photovoltaique utilisant ce substrat

Publications (2)

Publication Number Publication Date
EP1421630A2 EP1421630A2 (de) 2004-05-26
EP1421630B1 true EP1421630B1 (de) 2006-10-18

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EP01810840A Withdrawn EP1289025A1 (de) 2001-08-30 2001-08-30 Abscheidungsverfahren von einer Oxydschicht auf einem Substrat und dieses verwendende photovoltaische Zelle
EP02754092A Expired - Lifetime EP1421630B1 (de) 2001-08-30 2002-08-23 Abscheidungsverfahren von einer oxydschicht auf einem substrat und dieses verwendende photovoltaische zelle

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EP01810840A Withdrawn EP1289025A1 (de) 2001-08-30 2001-08-30 Abscheidungsverfahren von einer Oxydschicht auf einem Substrat und dieses verwendende photovoltaische Zelle

Country Status (8)

Country Link
US (1) US7390731B2 (de)
EP (2) EP1289025A1 (de)
JP (1) JP4491233B2 (de)
CN (1) CN1326255C (de)
AU (1) AU2002322952A1 (de)
DE (1) DE60215523T2 (de)
ES (1) ES2274069T3 (de)
WO (1) WO2003021690A2 (de)

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ATE364900T1 (de) * 2004-02-13 2007-07-15 Shell Solar Gmbh Einrichtung zum aufbringen einer flüssigen dotierungsstofflösung auf einem wafer
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JP4918224B2 (ja) * 2005-01-21 2012-04-18 昭和シェル石油株式会社 透明導電膜製膜装置及び多層透明導電膜連続製膜装置
US8197914B2 (en) 2005-11-21 2012-06-12 Air Products And Chemicals, Inc. Method for depositing zinc oxide at low temperatures and products formed thereby
EP1840966A1 (de) * 2006-03-30 2007-10-03 Universite De Neuchatel Transparente, leitende und strukturierte Schicht sowie Verfahren zu ihrer Herstellung
MY148287A (en) 2006-08-29 2013-03-29 Pilkington Group Ltd Method of making a low-resistivity, doped zinc oxide coated glass article and the coated glass article made thereby
US20080128022A1 (en) * 2006-11-15 2008-06-05 First Solar, Inc. Photovoltaic device including a tin oxide protective layer
DE102006062019A1 (de) * 2006-12-29 2008-07-03 Näbauer, Anton, Dr. Verfahren zur Herstellung von mechanisch stabilen Dünnschicht Photovoltaik Solarmodulen unter Verwendung von Glas
US8203071B2 (en) 2007-01-18 2012-06-19 Applied Materials, Inc. Multi-junction solar cells and methods and apparatuses for forming the same
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WO2010151430A1 (en) 2009-06-22 2010-12-29 Arkema Inc. Chemical vapor deposition using n,o polydentate ligand complexes of metals
JP5508800B2 (ja) * 2009-09-30 2014-06-04 株式会社カネカ 薄膜の製造方法、並びに、太陽電池の製造方法
US8525019B2 (en) 2010-07-01 2013-09-03 Primestar Solar, Inc. Thin film article and method for forming a reduced conductive area in transparent conductive films for photovoltaic modules
WO2012031102A2 (en) 2010-09-03 2012-03-08 Corning Incorporated Thin film silicon solar cell in multi-junction configuration on textured glass
US8906732B2 (en) * 2010-10-01 2014-12-09 Stion Corporation Method and device for cadmium-free solar cells
US8628997B2 (en) * 2010-10-01 2014-01-14 Stion Corporation Method and device for cadmium-free solar cells
DE102015215434A1 (de) * 2015-08-13 2017-02-16 Fraunhofer-Gesellschaft zur Förderung der angewandten Forschung e.V. Verfahren zur Abscheidung dünner Schichten

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Publication number Publication date
DE60215523T2 (de) 2007-06-21
US7390731B2 (en) 2008-06-24
JP2005501182A (ja) 2005-01-13
DE60215523D1 (de) 2006-11-30
US20040235286A1 (en) 2004-11-25
EP1289025A1 (de) 2003-03-05
AU2002322952A1 (en) 2003-03-18
JP4491233B2 (ja) 2010-06-30
WO2003021690A3 (fr) 2003-11-06
CN1550045A (zh) 2004-11-24
CN1326255C (zh) 2007-07-11
ES2274069T3 (es) 2007-05-16
WO2003021690A2 (fr) 2003-03-13
EP1421630A2 (de) 2004-05-26

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